Definitely Species 8472 (the Borg were losing to them!), although they were short lived in the series. Next to them, definitely the Borg... although I still feel the whole "queen" bit destroyed an important menacing aspect to the Borg. That "faceless collective" was ominous. Just watch that first encounter in TNG... it reminds you of how horrifying these creatures were, before being more "humanized" with a queen leader.
One thing that really pissed me off about Enterprise was the introduction of the Borg. Total canon violation. No need for it. But I guess with the dire ratings problem, they couldn't resist leveraging them. Origin totally belongs to TNG and that should never have been "rewritten."